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Dehydrogenation of ...
Dehydrogenation of Propane and n-Butane Catalyzed by Isolated PtZn4 Sites Supported on Self-Pillared Zeolite Pentasil Nanosheets
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- Qi, Liang (författare)
- Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA.;Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA.;Chinese Acad Sci, Dalian Inst Chem Phys, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China.
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- Zhang, Yanfei (författare)
- Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA.;Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA.
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- Babucci, Melike (författare)
- Uppsala universitet,Solcellsteknik,Univ Calif Davis, Dept Chem Engn, Davis, CA 95616 USA.
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- Chen, Cailing (författare)
- King Abdullah Univ Sci & Technol KAUST, Adv Membranes & Porous Mat AMPM Ctr, Phys Sci & Engn Div, Thuwal 239556900, Saudi Arabia.;KAUST, KAUST Catalysis Ctr KCC, Thuwal 239556900, Saudi Arabia.
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- Lu, Peng (författare)
- Johns Hopkins Univ, Dept Chem & Biomol Engn, Baltimore, MD 21218 USA.;Johns Hopkins Univ, Inst NanoBioTechnol, Baltimore, MD 21218 USA.
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- Li, Jingwei (författare)
- Chongqing Univ, Multiscale Porous Mat Ctr, Inst Adv Interdisciplinary Studies, Chongqing 400044, Peoples R China.;Chongqing Univ, Sch Chem & Chem Engn, Chongqing 400044, Peoples R China.
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- Dun, Chaochao (författare)
- Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA.
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- Hoffman, Adam S. (författare)
- SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Light Source, Menlo Pk, CA 94025 USA.
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- Urban, Jeffrey J. (författare)
- Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA.
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- Tsapatsis, Michael (författare)
- Johns Hopkins Univ, Dept Chem & Biomol Engn, Baltimore, MD 21218 USA.;Johns Hopkins Univ, Inst NanoBioTechnol, Baltimore, MD 21218 USA.
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- Bare, Simon R. (författare)
- SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Light Source, Menlo Pk, CA 94025 USA.
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- Han, Yu (författare)
- King Abdullah Univ Sci & Technol KAUST, Adv Membranes & Porous Mat AMPM Ctr, Phys Sci & Engn Div, Thuwal 239556900, Saudi Arabia.;KAUST, KAUST Catalysis Ctr KCC, Thuwal 239556900, Saudi Arabia.
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- Gates, Bruce C. (författare)
- Chinese Acad Sci, Dalian Inst Chem Phys, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China.
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- Bell, Alexis T. (författare)
- Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA.;Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA.
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Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA;Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA.;Chinese Acad Sci, Dalian Inst Chem Phys, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China. Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA.;Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. (creator_code:org_t)
- 2022-08-31
- 2022
- Engelska.
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Ingår i: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 12:18, s. 11177-11189
- Relaterad länk:
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
Stäng
- Propene and 1,3-butadiene are important building-block chemicals that can be produced by dehydrogenation of propane and butane on Pt catalysts. A challenge is to develop highly active and selective catalysts that are resistant to deactivation by Pt sintering and coke formation. We have recently shown (Qi , J. Am. Chem. Soc. 2021, 143, 21364-21378) that these objectives can be met for propane dehydrogenation (PDH) using atomically dispersed Pt anchored to neighboring SiOZn-OH groups bonded to the framework of dealuminated zeolite BEA. In the present study, we demonstrate that significantly superior performance can be achieved using self-pillared pentasil (SPP) zeolite nanosheets as supports. Following catalyst reduction in H-2, atomic resolution, scanning transmission electron microscopy (STEM), and X-ray absorption spectroscopy (XAS) indicate that Pt is stabilized in structures well approximated as ( Si-O-Zn)(4-5)Pt. These species are highly active, selective, and stable for PDH to give propene and for n-butane dehydrogenation (BDH) to give 1,3-butadiene. No catalyst deactivation was observed after 12 days of time on stream, and the selectivity remained at nearly 100% for PDH conducted at 823 K and a weight hourly space velocity (WHSV) of 1350 h(-1). The apparent rate coefficient for PDH on this catalyst is significantly higher than that reported previously for Pt-containing catalysts. For BDH at 823 K and a WHSV of 3560 h(-1), the selectivity to butene isomers and 1,3-butadiene is 98.9%, and the selectivity to 1,3-butadiene is 45%. We propose that the high catalyst stability observed during PDH and BDH is a consequence of a large fraction of the Pt-containing centers being located on the external surface of the zeolite nanosheets, where nascent coke precursors can desorb before condensing to form coke.
Ämnesord
- NATURVETENSKAP -- Kemi -- Materialkemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Materials Chemistry (hsv//eng)
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Nyckelord
- catalytic dehydrogenation
- light alkane
- isolated PtZn4
- zeolite nanosheet
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Qi, Liang
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Zhang, Yanfei
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Babucci, Melike
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Chen, Cailing
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Lu, Peng
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Li, Jingwei
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Dun, Chaochao
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Hoffman, Adam S.
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Urban, Jeffrey J ...
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Tsapatsis, Micha ...
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Bare, Simon R.
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Han, Yu
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Gates, Bruce C.
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Bell, Alexis T.
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- NATURVETENSKAP
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NATURVETENSKAP
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och Kemi
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och Materialkemi
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- NATURVETENSKAP
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NATURVETENSKAP
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och Kemi
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ACS Catalysis
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Uppsala universitet